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Enhanced peroxymonosulfate activation by supported microporous carbon for degradation of tetracycline via non-radical mechanism
Separation and Purification Technology ( IF 8.6 ) Pub Date : 2020-01-25 , DOI: 10.1016/j.seppur.2020.116617
Jia Li , Jialu Zhu , Lizhu Fang , Yulun Nie , Na Tian , Xike Tian , Liqiang Lu , Zhaoxin Zhou , Chao Yang , Yong Li

Carbon-based peroxymonosulfate (PMS) activator as a promising candidate for substituting metal-based heterogeneous catalysts has drawn increasing concerns. In this study, we reported two supported microporous carbon based PMS activators after treatment by KOH and ZnCl2 (denoted as SMC-K and SMC-Z). Their catalytic activity was evaluated and compared by the degradation efficiency of a typical antibiotics of tetracycline (TC). The results indicated that SMC-K exhibited a higher PMS activation performance than SMC-Z. TC degradation data followed the pseudo-first-order kinetics with reaction rate constants of 0.0818 and 0.0392 min-1, respectively. Based on the characterization results, SMC-K had an extensive microporous structure with abundant vacancy defects and catalytic active sites, accompanied by more basic site distribution. The PMS activation mechanism was further explored via quenching tests, electron paramagnetic resonance (EPR) and electrochemical impedance spectroscopy (EIS). TC degradation occurred via a non-radical oxidation mechanism: (1) direct oxidation by activated PMS where SMC-K acted as the electron transfer shuttle, (2) oxidized by 1O2 instead of SO4•- or OH generated from PMS self-decomposition. Furthermore, a reasonable degradation pathway of TC based on the non-radical oxidation has been proposed. This work benefits to develop new treatment technologies for organic pollutants removal in practical application.



中文翻译:

负载的微孔碳增强的过氧单硫酸盐活化,通过非自由基机理降解四环素

碳基过氧单硫酸盐(PMS)活化剂作为取代金属基非均相催化剂的有前途的候选者引起了越来越多的关注。在这项研究中,我们报道了两种受支持的微孔碳基PMS活化剂,经KOH和ZnCl 2处理(表示为SMC-K和SMC-Z)。通过典型的四环素抗生素(TC)的降解效率评估并比较了它们的催化活性。结果表明,SMC-K具有比SMC-Z更高的PMS激活性能。TC降解数据遵循拟一级动力学,反应速率常数为0.0818和0.0392 min -1, 分别。根据表征结果,SMC-K具有广泛的微孔结构,具有大量的空位缺陷和催化活性位,并伴随着更多的基本位点分布。通过猝灭测试,电子顺磁共振(EPR)和电化学阻抗谱(EIS)进一步探索了PMS激活机制。TC降解是通过非自由基氧化机理发生的:(1)活化的PMS直接氧化,其中SMC-K充当电子传递梭,(2)被1 O 2代替SO 4 •-氧化PMS自分解产生的OH。此外,已经提出了基于非自由基氧化的TC的合理降解途径。这项工作有益于开发在实际应用中用于去除有机污染物的新处理技术。

更新日期:2020-01-26
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